Impact of Heatwaves and Declining NOx on Nocturnal Monoterpene Oxidation in the Urban Southeastern United States

摘要

Abstract Nighttime oxidation of monoterpenes (MT) via the nitrate radical (NO3) and ozone (O3) contributes to the formation of secondary organic aerosol (SOA). This study uses observations in Atlanta, Georgia from 2011 to 2022 to quantify trends in nighttime production of NO3 (PNO3) and O3 concentrations and compare to model outputs from the EPA's Air QUAlity TimE Series Project (EQUATES). We present urban‐suburban gradients in nighttime NO3 and O3 concentrations and quantify their fractional importance (F) for MT oxidation. Both observations and EQUATES show a decline in PNO3, with modeled PNO3 declining faster than observations. Despite decreasing PNO3, we find that NO3 continues to dominate nocturnal boundary layer (NBL) MT oxidation (FNO3 = 60) in 2017, 2021, and 2022, which is consistent with EQUATES (FNO3 = 80) from 2013 to 2019. This contrasts an anticipated decline in FNO3 based on prior observations in the nighttime residual layer, where O3 is the dominant oxidant. Using two case studies of heatwaves in summer 2022, we show that extreme heat events can increase NO3 concentrations and FNO3, leading to short MT lifetimes (<1 hr) and high gas‐phase organic nitrate production. Regardless of the presence of heatwaves, our findings suggest sustained organic nitrate aerosol formation in the urban SE US under declining NOx emissions, and highlight the need for improved representation of extreme heat events in chemistry‐transport models and additional observations along urban to rural gradients.